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Covalent Organic Frameworks with Carbon-centered Radical Sites for Promoting the 4e- Oxygen Reduction Reaction.
Angew Chem Int Ed Engl
January 2025
Institute of Materials Research and Engineering, Sensor and Flexible Electronics, 2 Fusionopolis Way, 138634, SINGAPORE.
Radical covalent organic frameworks (RCOFs) have demonstrated significant potential in redox catalysis and energy conversion applications. However, the synthesis of stable RCOFs with well-defined neutral carbon radical centers is challenging due to the inherent radical instability, limited synthetic methods and characterization difficulties. Building upon the understanding of stable carbon radicals and structural modulations for preparing crystalline COFs, herein we report the synthesis of a crystalline carbon-centered RCOF through a facile post-oxidation process.
View Article and Find Full Text PDFThe Carbene Chemistry of -Sulfonyl Hydrazones: The Past, Present, and Future.
Chem Rev
January 2025
Department of Chemistry, Northeast Normal University, Changchun 130024, China.
-Sulfonyl hydrazones have been extensively used as operationally safe carbene precursors in modern organic synthesis due to their ready availability, facile functionalization, and environmental benignity. Over the past two decades, there has been tremendous progress in the carbene chemistry of -sulfonyl hydrazones in the presence of transition metal catalysts, under metal-free conditions, or using photocatalysts under photoirradiation conditions. Many carbene transfer reactions of -sulfonyl hydrazones are unique and cannot be achieved by any alternative methods.
View Article and Find Full Text PDFAccessing Azetidines through Magnesium-Mediated Nitrogen Group Transfer from Iminoiodinane to Donor-Acceptor Cyclopropanes.
Angew Chem Int Ed Engl
January 2025
New York University, Chemistry, 29 Washington Place, RM 10001, 10003, New York, UNITED STATES OF AMERICA.
Herein, we report a Lewis acid-mediated ring expansion of donor-acceptor cyclopropanes (DACs) to substituted azetidines via nucleophilic nitrogen group transfer from readily accessible iminoiodinane. This protocol operates under mild, transition-metal-free conditions, and showcases excellent chemoselectivity, along with broad functional group tolerance. We report for the first time that challenging alkyl donor-acceptor cyclopropanes can undergo ring expansion leading to aliphatic azetidines without relying on external oxidants or precious transition-metal catalysts.
View Article and Find Full Text PDFIntegrating Ni(OH) Nanoparticles on CdS for Efficient Noble-Metal-Free Photocatalytic H Evolution.
Molecules
December 2024
School of Pharmaceutical Sciences, Gannan Medical University, Ganzhou 341000, China.
Photocatalytic hydrogen evolution using inexhaustible clean solar energy is considered as a promising strategy. In order to build an efficient photocatalytic hydrogen production system to satisfy the demands of practical applications, it is of great significance to design photocatalysts that offer high activity, low cost, and high stability. Herein, a series of cheap CdS/Ni(OH) composite photocatalysts were designed and synthesized using the hydrothermal method.
View Article and Find Full Text PDFHighly efficient metal-free electrochemical membrane enables zero-valent sulfur recovery from thiourea wastewater.
Water Res
January 2025
School of Science, RMlT University, Melbourne, VC 3000. Australia.
Electrochemical recovery of zero-valent sulfur (S) from thiourea (TU) wastewater offers a promising waste-to-value strategy that expects to promote the sulfur resource cycle in water treatment but still suffer from electrode poisoning and sulfur over-oxidation. Herein, we designed a metal-free CNT electrochemical membrane for selective oxidation of thiourea and recovery of S. We found that defect sites on the carbon nanotube surface enable direct electron transfer for thiourea oxidation and may form carbon-sulfur bridge bonds, thereby facilitating the generation of S and urea.
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